C60-Bodipy hybrids exhibiting strong absorption of visible light and long-lived triplet excited states were used as photocatalysts for tandem oxidation/[3+2] cycloaddition of tetrahydroisoquinoline with N-phenylmaleimide to produce pyrrolo[2,1-a]isoquinolines. The reaction is substantially accelerated, compared to that catalyzed by Ru(bpy)3Cl2.